Johansson J Olof, Henderson Gordon G, Campbell Eleanor E B
EaStCHEM, School of Chemistry, University of Edinburgh , Edinburgh EH9 3JJ, U.K.
J Phys Chem A. 2014 Sep 18;118(37):8067-73. doi: 10.1021/jp408147f. Epub 2013 Nov 14.
Gas-phase fullerenes emit thermal electrons after femtosecond laser excitation in the wavelength range 400-800 nm. We have used angular-resolved photoelectron spectroscopy (PES) to study the influence of the laser's electric field on the dynamics of the thermally emitted electrons. The laser field introduces an asymmetry in the thermal electron distributions with respect to the laser polarization direction, which was confirmed by carrying out experiments at different wavelengths. A simple model could reproduce the trends in measured apparent temperatures in the PES. The asymmetry effect was exploited in a pump-probe experiment to estimate the time scale for thermal electron emission. It was found that, when 400 nm, 120 fs laser pulses of 2 TW cm(-2) intensity are used, thermal electrons are emitted up to ca. 300 fs after the peak of the laser pulse. The pump-probe scheme should be applicable to a wider range of complex molecules and clusters showing thermal electron emission on a femtosecond time scale.
气相富勒烯在400 - 800纳米波长范围内的飞秒激光激发后会发射热电子。我们使用角分辨光电子能谱(PES)来研究激光电场对热发射电子动力学的影响。激光场在热电子分布相对于激光偏振方向上引入了不对称性,这通过在不同波长下进行实验得到了证实。一个简单的模型可以重现PES中测量的表观温度趋势。在泵浦 - 探测实验中利用了这种不对称效应来估计热电子发射的时间尺度。结果发现,当使用强度为2 TW cm⁻²的400纳米、120飞秒激光脉冲时,热电子在激光脉冲峰值后约300飞秒内发射。泵浦 - 探测方案应适用于更广泛的在飞秒时间尺度上表现出热电子发射的复杂分子和团簇。